Self‐Powered Microscale Pumps Based on Analyte‐Initiated Depolymerization Reactions

Zhang, Hua; Yeung, Kimy; Robbins, Jessica S.; Pavlick, Ryan A.; Wu, Meng; Liu, Ran; Sen, Ayusman; Phillips, Scott T.

doi:10.1002/anie.201107787

Cited by 92 publications

(88 citation statements)

References 36 publications

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“…These polymers include poly(benzyl carbamates) [Figure (a)], poly(benzyl ethers) [Figure (b)], and polymers that depolymerize via alternating intramolecular cyclization/quinone methide elimination reactions [Figure (c)] . The two other classes offer unique mechanisms of depolymerization from one another as well as from the first three classes of polymers: they depolymerize via intramolecular cyclization reactions [Figure (d)] or acetal chemistry [Figure (e)] . There is vast chemical space yet to be explored.…”

Section: Current Classes Of Cdr Polymersmentioning

confidence: 99%

“…The final class of CD r polymers is poly(phthalaldehyde) (PPA) that contains a reaction‐based detection unit on either end of the polymer, or on both ends [Figure (e)] . These polymers typically are prepared via low temperature (−78°C) anionic cyclopolymerization of 1,2‐aromatic dialdehydes (a reaction‐based detection unit can serve as the initiator), followed by quenching of the reaction by addition of an electrophilic reagent, which oftentimes is a reaction‐based detection unit .…”

Section: Current Classes Of Cdr Polymersmentioning

confidence: 99%

“…In fact, several proof‐of‐concept studies are already beginning to reveal these capabilities. For example, CD r polymers have been used to make (i) stimuli‐responsive, non‐mechanical pumps; (ii) micellar aggregates, polymersomes, and micro‐ and nanocapsules for controlled release applications; and (iii) shape‐changing and vanishing plastics. They also have been used as signal amplification reagents in the context of point‐of‐care diagnostics .…”

Section: Introductionmentioning

confidence: 99%

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Amplified responses in materials using linear polymers that depolymerize from end‐to‐end when exposed to specific stimuli

Phillips

Robbins

DiLauro

et al. 2014

J of Applied Polymer Sci

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This review describes new types of smart materials that have the dual capabilities of responding to selective signals and providing an amplified response. Amplification arises from a signal-induced depolymerization reaction, where a single signaling event causes an entire polymer to convert to small molecules. When incorporated into a material, depolymerization of these polymers causes a change in shape, internal structure, or surfaces properties of the material. Moreover, the small molecules arising from depolymerization can play a role in the amplified response, particularly when they provide a secondary function (e.g., production of color or fluorescence). A brief overview of the current examples of linear depolymerizable polymers is provided, as are representative proof-of-concept applications of these polymers in the context of diagnostics and materials that remodel themselves and/or their surroundings. Together, these examples highlight the potential of this new class of polymers to provide unique and dramatic function to stimuli-responsive materials.

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Section: Current Classes Of Cdr Polymersmentioning

confidence: 99%

Section: Current Classes Of Cdr Polymersmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

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Amplified responses in materials using linear polymers that depolymerize from end‐to‐end when exposed to specific stimuli

Phillips

Robbins

DiLauro

et al. 2014

J of Applied Polymer Sci

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“…Moreover, the fabrication technique is exceptionally mild and thus enables the formation of core−shell microcapsules using sensitive depolymerizable polymers such as poly(phthalaldehyde) (PPHA) (Figure 1). 16,17 Herein we demonstrate these concepts by fabricating model stimuli-responsive core−shell microcapsules using PPHA that contains a fluoride-responsive endcap. The end-cap controls the stability and reactivity of the PPHA polymer and thus enables release of the contents of the capsules selectively when exposed to fluoride (a model stimulus), even in aqueous media.…”

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confidence: 97%

Stimuli-Responsive Core–Shell Microcapsules with Tunable Rates of Release by Using a Depolymerizable Poly(phthalaldehyde) Membrane

et al. 2013

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Flow-focusing microfluidic techniques were used to provide access to core−shell microcapsules in which the shell is composed of end-capped poly(phthalaldehydes) that depolymerize completely from head-to-tail in response to fluoride. Microcapsules made from these depolymerizable polymers provide an amplified response to the applied chemical signal, where the rate of the response can be tuned both by varying the length of the polymer and the thickness of the shell wall. ■ INTRODUCTIONStimuli-responsive polymeric core−shell microcapsules are promising materials for controlled release applications. 1−8 Capsules of this type typically release their contents either through induced chemical changes in the polymers that compose the shell or via bulk structural changes to the shell wall. 1 These traditional triggered-release strategies provide responses that are nonamplified: i.e., a single membrane−signal interaction produces one small structural change in the shell wall, whereas release occurs only after many signals have reacted with and altered the shell wall. In contrast, a new release strategy has emerged where shell walls are formed from polymers that depolymerize continuously and completely from head-to-tail when an appropriate signal is detected by the polymer. 1,9 This depolymerization reaction provides an amplified response that, in theory, increases the sensitivity of the capsules as well as their rate of response once the appropriate signal is detected. Despite these favorable attributes, however, only one example of a stimuli-responsive core−shell polymeric microcapsule made from a head-to-tail depolymerizable polymer has been demonstrated to date, 10 with additional related examples demonstrated in responsive nanocapsules and micelles. 11,12 Further development of this depolymerizable shell wall concept has been hindered by the limited number of polymers that are capable of depolymerizing from head-to-tail in response to a specific signal, as well as by substantial challenges in fabricating core−shell microcapsules using polymers that are primed to depolymerize.In this article, we describe the use of flow-focusing microfluidic strategies for fabricating these types of depolymerizable core−shell microcapsules. 13−15 This technique is highly reproducible, readily forms capsules that contain aqueous interiors, is capable of generating capsules that can be suspended in an aqueous solution that differs from the solution within the capsule, and does not require synthetic manipulation of the polymer for incorporation into the shell wall. Moreover, the fabrication technique is exceptionally mild and thus enables the formation of core−shell microcapsules using sensitive depolymerizable polymers such as poly(phthalaldehyde) (PPHA) (Figure 1). 16,17 Herein we demonstrate these concepts by fabricating model stimuli-responsive core−shell microcapsules using PPHA that contains a fluoride-responsive endcap. The end-cap controls the stability and reactivity of the PPHA polymer and thus enables release of the ...

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“…Recent developments have also included micropumps that are independent of the substrate materials, utilizing depolymerization reactions upon introduction of external stimuli, such as using chemical and ultraviolet factors. [38] Further manipulation of the fluid-flow directions can be accomplished by changing the fuel source [39] or the zeta potential of the particle and the micropump's surface. [40] Depolymerization to reactive monomers that can remove inorganics from the solution are particularly interesting owing to the amplification provided by the catalytic reactions.…”

Section: Immobilized Micromotors: Micropumpsmentioning

confidence: 99%

Chemical Energy Powered Nano/Micro/Macromotors and the Environment

Moo

Pumera

2014

Chemistry A European J

164

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The rise of miniaturized artificial self-powered devices, demonstrating autonomous motion, has brought in new considerations from the environmental perspective. This review addresses the interplay between these nano/micro/macromotors and the environment, recent advances, and their applications in pollution management. Such self-propelled devices are able to actuate chemical energy into mechanical motion in situ, adding another powerful dimension towards solving environmental problems. Use of synthetic nano/micro/macromotors has demonstrated potential in environmental remediation, both in pollutant removal and contaminant degradation, owing to motion-induced mixing. At the same time, the chemical environment exerts influence on the locomotion of the motors. These sensitized self-powered devices demonstrate capabilities for being deployed as sensors and their chemotactic behaviors show efficacy to act as first responders towards a chemical leakage. Thus, the notion of a self-propelling entity also entails further investigation into its inherent toxicity and possible implications as a pollutant. Future challenges and outlook of the use of these miniaturized devices are discussed, with specific regard to the fields of environmental remediation and monitoring, as we move towards their wider acceptance. We believe that these tiny machines will stand up to the task as solutions for environmental sustainability in the 21st century.

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Self‐Powered Microscale Pumps Based on Analyte‐Initiated Depolymerization Reactions

Cited by 92 publications

References 36 publications

Amplified responses in materials using linear polymers that depolymerize from end‐to‐end when exposed to specific stimuli

Amplified responses in materials using linear polymers that depolymerize from end‐to‐end when exposed to specific stimuli

Stimuli-Responsive Core–Shell Microcapsules with Tunable Rates of Release by Using a Depolymerizable Poly(phthalaldehyde) Membrane

Chemical Energy Powered Nano/Micro/Macromotors and the Environment

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